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Suso signed for Liverpool in the summer of 2010 from his hometown club Cadiz. He rejected offers from Barcelona and Real Madrid in the process, later saying "I was going to sign for Real Madrid but one day before it the phone rang and Rafael Benitez spoke to me. He convinced me that Liverpool was the club for me and after that I had to change my plans. I was going to come to Liverpool."

Suso made an appearance for the first team in a pre-season friendly against Borussia Mönchengladbach on 1 August 2010, and he also took part in Jamie Carragher's testimonial match on 4 September 2010. However for competitive fixtures, he was immediately placed in the Reserve team, foregoing the Academy. In the 2010-11 season, he made the joint-highest number of appearances for the side with 17, and netted three goals as he adapted well to life on Merseyside. He followed this up with five goals in 17 League games during the 2011-12 Reserves season and he also added seven appearances in the NextGen Series to his name. Suso was awarded with the first team squad number 30 for the 2011-12 season and he frequently trained with the first team at Melwood.

In July 2012, Suso was invited to take part in Liverpool's pre-season tour of the USA. He linked up with his teammates just two days after winning the Under 19 European Championships with Spain. He appeared in the second half of the friendly match versus Toronto, and impressed with his all-round dangerous play and impressive shooting.

He made his Liverpool debut on 20 September 2012 in a 5-3 win over Swiss team Young Boys in the Europa League group match. He then made his debut in the League on 23 September in a home game against Manchester United, coming on at half-time in place of Fabio Borini and was immediately involved in putting his side in front. On 29 September 2012, Suso was handed his first start in a League game away to Norwich. The match finished 5-2 to Liverpool as Suso played the first hour of the match. Having made an encouraging start to his first team career, the Liverpool fans could be heard vociferously chanting his name as he left the pitch. Prior to the game, manager Brendan Rodgers had spoken of how impressed he had been with Suso, and confirmed the club were looking to tie the Spaniard down to a new long term contract with his deal set to expire in the summer of 2013.

Suso signed his new contract on 19 October 2012. Upon signing, he stated "I am really happy. Liverpool are one of the biggest clubs in the world and this is the right place for me. I am happy Brendan has shown trust in me. I had no questions about signing a new deal and I am really glad to have done so. This is one of the best days of my life." Manager Brendan Rodgers said of Suso's signing "We are all delighted Suso has committed his long-term future to Liverpool Football Club. At 18, he has demonstrated outstanding technical qualities but also shown very good temperament to play for such a prestigious club."

As the season progressed, the return to form of Stewart Downing and the purchases of forwards Daniel Sturridge and Philippe Coutinho limited Suso's opportunities with the first team. After some speculation he would make a loan move from the club in the January 2013 transfer window, Suso began appearing again for the Liverpool Under 21s in order to provide the Spaniard with game time. After the season's end, on 12 July 2013, Liverpool confirmed Suso had joined La Liga side Almeria on loan for the 2013-14 season.

He returned at the end of the season, and spoke if his desire to win a new contract at Liverpool and make a success of his career at Anfield. On 19 July 2014, Suso scored in Liverpool's pre-season match away at Preston, curling an impressive finish into the top corner, levelling the tie at 1-1 before the Reds went on to claim a 2-1 victory.

Suso made his first appearance of the 2014-15 season on 23 September 2014, appearing as a second half substitute in Liverpool's League Cup clash with Middlesbrough. With the score level at 1-1, the game went to extra time and Suso netted to put Liverpool 2-1 up- striking a loose ball from 12 yards out into the centre of the net. He played well in his cameo and netted two of Liverpool's spot kicks in the penalty shootout after Boro had levelled the tie in regulation time. The Kop could be heard vociferously chanting his name as he went to take his penalties.

Injury kept Suso sidelined for the rest of Liverpool's matches in 2014, and in January 2015, reports were rife that Suso had signed a pre-contract agreement with AC Milan and would move to the club in the summer. AC Milan moved to take Suso in the January transfer window for a nominal fee instead, bringing an end to his five year association with the Reds.

Suso's playing style has been likened to such stars as Manchester City's David Silva and Barcelona's Andres Iniesta. He is a tricky, technically gifted attacking midfielder who likes to drop in behind the strikers and can busy opposition defences with flair and ingenuity. He also has the ability sit deep and dictate the pace of games using both a long and short range of passing. In the 2011-12 season however, Suso was utilised more on the right wing by the Reserves, making use of his ability to cut inside and use his cultured left foot for shots. It took him time to adapt to this new role, though he did eventually grow into it well.